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Long-term (2001–2012) concentrations of fine particulate matter (PM2.5) and the impact on human health in Beijing, China

Beijing, the capital of China, is a densely populated city with poor air quality. The impact of high pollutant concentrations, in particular of aerosol particles, on human health is of major concern. The present study uses aerosol optical depth (AOD) as proxy to estimate long-term PM2.5 and subsequently estimates the premature mortality due to PM2.5. We use the AOD from 2001 to 2012 from the Aerosol Robotic Network (AERONET) site in Beijing and the ground-based PM2.5 observations from the US embassy in Beijing from 2010 to 2011 to establish a relationship between PM2.5 and AOD. By including the atmospheric boundary layer height and relative humidity in the comparative analysis, the correlation (R2) increases from 0.28 to 0.62. We evaluate 12 years of PM2.5 data for the Beijing central area using an estimated linear relationship with AOD and calculate the yearly premature mortality by different diseases attributable to PM2.5. The estimated average total mortality due to PM2.5 is about 5100 individuals per year for the period 2001–2012 in the Beijing central area, and for the period 2010–2012 the per capita mortality for all ages due to PM2.5 is around 15 per 10 000 person-years, which underscores the urgent need for air pollution abatement.
Using the OMI aerosol index and absorption aerosol optical depth to evaluate the NASA MERRA Aerosol Reanalysis

A radiative transfer interface has been developed to simulate the UV aerosol index (AI) from the NASA Goddard Earth Observing System version 5 (GEOS-5) aerosol assimilated fields. The purpose of this work is to use the AI and aerosol absorption optical depth (AAOD) derived from the Ozone Monitoring Instrument (OMI) measurements as independent validation for the Modern Era Retrospective analysis for Research and Applications Aerosol Reanalysis (MERRAero). MERRAero is based on a version of the GEOS-5 model that is radiatively coupled to the Goddard Chemistry, Aerosol, Radiation, and Transport (GOCART) aerosol module and includes assimilation of aerosol optical depth (AOD) from the Moderate Resolution Imaging Spectroradiometer (MODIS) sensor. Since AI is dependent on aerosol concentration, optical properties and altitude of the aerosol layer, we make use of complementary observations to fully diagnose the model, including AOD from the Multi-angle Imaging SpectroRadiometer (MISR), aerosol retrievals from the AErosol RObotic NETwork (AERONET) and attenuated backscatter coefficients from the Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observation (CALIPSO) mission to ascertain potential misplacement of plume height by the model. By sampling dust, biomass burning and pollution events in 2007 we have compared model-produced AI and AAOD with the corresponding OMI products, identifying regions where the model representation of absorbing aerosols was deficient. As a result of this study over the Saharan dust region, we have obtained a new set of dust aerosol optical properties that retains consistency with the MODIS AOD data that were assimilated, while resulting in better agreement with aerosol absorption measurements from OMI. The analysis conducted over the southern African and South American biomass burning regions indicates that revising the spectrally dependent aerosol absorption properties in the near-UV region improves the modeled-observed AI comparisons. Finally, during a period where the Asian region was mainly dominated by anthropogenic aerosols, we have performed a qualitative analysis in which the specification of anthropogenic emissions in GEOS-5 is adjusted to provide insight into discrepancies observed in AI comparisons.
Photochemical aging of volatile organic compounds associated with oil and natural gas extraction in the Uintah Basin, UT, during a wintertime ozone formation event

High concentrations of volatile organic compounds (VOCs) associated with oil and natural gas extraction were measured during a strong temperature inversion in the winter of 2013 at a rural site in the Uintah Basin, Utah. During this period, photochemistry enhanced by the stagnant meteorological conditions and concentrated VOCs led to high ozone mixing ratios (150 ppbv). A simple analysis of aromatic VOCs measured by proton-transfer-reaction mass-spectrometry (PTR-MS) is used to estimate (1) VOC emission ratios (the ratio of two VOCs at the time of emission) relative to benzene, (2) aromatic VOC emission rates, and (3) ambient OH radical concentrations. These quantities are determined from a best fit to VOC : benzene ratios as a function of time. The main findings are that (1) emission ratios are consistent with contributions from both oil and gas producing wells; (2) the emission rate of methane (27–57 × 103 kg methane h−1), extrapolated from the emission rate of benzene (4.1 ± 0.4 × 105 molecules cm−3 s−1), agrees with an independent estimate of methane emissions from aircraft measurements in 2012; and (3) calculated daily OH concentrations are low, peaking at 1 × 106 molecules cm−3, and are consistent with Master Chemical Mechanism (MCM) modeling. The analysis is extended to photochemical production of oxygenated VOCs measured by PTR-MS and is able to explain daytime variability of these species. It is not able to completely reproduce nighttime behavior, possibly due to surface deposition. Using results from this analysis, the carbon mass of secondary compounds expected to have formed by the sixth day of the stagnation event was calculated, then compared to the measured mass of primary and secondary compounds. Only 17% of the expected secondary carbon mass is accounted for by gas phase, aerosol, and snow organic carbon measurements. The disparity is likely due to substantial amounts of unquantified oxygenated products.
Diurnal variations of aerosol optical properties in the North China Plain and their influences on the estimates of direct aerosol radiative effect

In this paper, the diurnal variations of aerosol optical properties and their influences on the estimation of daily average direct aerosol radiative effect (DARE) in the North China Plain (NCP) are investigated based on in situ measurements from Haze in China campaign. For ambient aerosol, the diurnal patterns of single scattering albedo (SSA) and asymmetry factor (g) in the NCP are both highest at dawn and lowest in the late afternoon, and quite different from those of dry-state aerosol. The relative humidity (RH) is the dominant factor which determines the diurnal pattern of SSA and g for ambient aerosol. Basing on the calculated SSA and g, several cases are designed to investigate the impacts of the diurnal changes of aerosol optical properties on DARE. The results demonstrate that the diurnal changes of SSA and g in the NCP have significant influences on the estimation of DARE at the top of the atmosphere (TOA). If the full temporal coverage of aerosol optical depth (AOD), SSA and g are available, an accurate estimation of daily average DARE can be achieved by using the daily averages of AOD, SSA and g. However, due to the lack of full temporal coverage data sets of SSA and g, their daily averages are usually not available. Basing on the results of designed cases, if the RH plays a dominant role in the diurnal variations of SSA and g, we suggest that using both SSA and g averaged over early morning and late afternoon as inputs for radiative transfer model to improve the accurate estimation of DARE. If the temporal samplings of SSA or g are too few to adopt this method, either averaged over early morning or late afternoon of both SSA and g can be used to improve the estimation of DARE at the TOA.
Modeling the formation and aging of secondary organic aerosols in Los Angeles during CalNex 2010

Four different literature parameterizations for the formation and evolution of urban secondary organic aerosol (SOA) frequently used in 3-D models are evaluated using a 0-D box model representing the Los Angeles metropolitan region during the California Research at the Nexus of Air Quality and Climate Change (CalNex) 2010 campaign. We constrain the model predictions with measurements from several platforms and compare predictions with particle- and gas-phase observations from the CalNex Pasadena ground site. That site provides a unique opportunity to study aerosol formation close to anthropogenic emission sources with limited recirculation. The model SOA that formed only from the oxidation of VOCs (V-SOA) is insufficient to explain the observed SOA concentrations, even when using SOA parameterizations with multi-generation oxidation that produce much higher yields than have been observed in chamber experiments, or when increasing yields to their upper limit estimates accounting for recently reported losses of vapors to chamber walls. The Community Multiscale Air Quality (WRF-CMAQ) model (version 5.0.1) provides excellent predictions of secondary inorganic particle species but underestimates the observed SOA mass by a factor of 25 when an older VOC-only parameterization is used, which is consistent with many previous model–measurement comparisons for pre-2007 anthropogenic SOA modules in urban areas. Including SOA from primary semi-volatile and intermediate-volatility organic compounds (P-S/IVOCs) following the parameterizations of Robinson et al. (2007), Grieshop et al. (2009), or Pye and Seinfeld (2010) improves model–measurement agreement for mass concentration. The results from the three parameterizations show large differences (e.g., a factor of 3 in SOA mass) and are not well constrained, underscoring the current uncertainties in this area. Our results strongly suggest that other precursors besides VOCs, such as P-S/IVOCs, are needed to explain the observed SOA concentrations in Pasadena. All the recent parameterizations overpredict urban SOA formation at long photochemical ages (≈ 3 days) compared to observations from multiple sites, which can lead to problems in regional and especially global modeling. However, reducing IVOC emissions by one-half in the model to better match recent IVOC measurements improves SOA predictions at these long photochemical ages. Among the explicitly modeled VOCs, the precursor compounds that contribute the greatest SOA mass are methylbenzenes. Measured polycyclic aromatic hydrocarbons (naphthalenes) contribute 0.7% of the modeled SOA mass. The amounts of SOA mass from diesel vehicles, gasoline vehicles, and cooking emissions are estimated to be 16–27, 35–61, and 19–35%, respectively, depending on the parameterization used, which is consistent with the observed fossil fraction of urban SOA, 71(±3) %. The relative contribution of each source is uncertain by almost a factor of 2 depending on the parameterization used. In-basin biogenic VOCs are predicted to contribute only a few percent to SOA. A regional SOA background of approximately 2.1 μg m−3 is also present due to the long-distance transport of highly aged OA, likely with a substantial contribution from regional biogenic SOA. The percentage of SOA from diesel vehicle emissions is the same, within the estimated uncertainty, as reported in previous work that analyzed the weekly cycles in OA concentrations (Bahreini et al., 2012; Hayes et al., 2013). However, the modeling work presented here suggests a strong anthropogenic source of modern carbon in SOA, due to cooking emissions, which was not accounted for in those previous studies and which is higher on weekends. Lastly, this work adapts a simple two-parameter model to predict SOA concentration and O/C from urban emissions. This model successfully predicts SOA concentration, and the optimal parameter combination is very similar to that found for Mexico City. This approach provides a computationally inexpensive method for predicting urban SOA in global and climate models. We estimate pollution SOA to account for 26 Tg yr−1 of SOA globally, or 17% of global SOA, one-third of which is likely to be non-fossil.
Measuring and modeling mercury in the atmosphere: a critical review

Mercury (Hg) is a global health concern due to its toxicity and ubiquitous presence in the environment. Here we review current methods for measuring the forms of Hg in the atmosphere and models used to interpret these data. There are three operationally defined forms of atmospheric Hg: gaseous elemental mercury (GEM), gaseous oxidized mercury (GOM), and particulate bound mercury (PBM). There is relative confidence in GEM measurements (collection on a gold surface), but GOM (collection on potassium chloride (KCl)-coated denuder) and PBM (collected using various methods) are less well understood. Field and laboratory investigations suggest the methods to measure GOM and PBM are impacted by analytical interferences that vary with environmental setting (e.g., ozone, relative humidity), and GOM concentrations measured by the KCl-coated denuder can be too low by a factor of 1.6 to 12 depending on the chemical composition of GOM. The composition of GOM (e.g., HgBr2, HgCl2, HgBrOH) varies across space and time. This has important implications for refining existing measurement methods and developing new ones, model/measurement comparisons, model development, and assessing trends. Unclear features of previously published data may now be re-examined and possibly explained, which is demonstrated through a case study. Priorities for future research include identification of GOM compounds in ambient air and development of information on their chemical and physical properties and GOM and PBM calibration systems. With this information, identification of redox mechanisms and associated rate coefficients may be developed.
Wind extraction potential from ensemble Kalman filter assimilation of stratospheric ozone using a global shallow water model

The feasibility of extracting wind information from stratospheric ozone observations is tested using ensemble Kalman filter (EnKF) data assimilation (DA) and a global shallow water model that includes advection of an ozone-like tracer. Simulated observations are created from a truth run (TR) that resembles the Northern Hemisphere winter stratosphere with a polar vortex disturbed by planetary-scale wave forcing. Ozone observations mimic sampling of a polar-orbiting satellite, while geopotential height observations are randomly placed in space and time. EnKF experiments are performed assimilating ozone, height, or both, over a 10-day period. The DA is also implemented using two different pairs of flow variables: zonal and meridional wind (EnKF-uv) and stream function and velocity potential (EnKF-ψχ). Each experiment is tuned for optimal localization length, while the ensemble spread is adaptively inflated using the TR. The experiments are evaluated using the maximum wind extraction potential (WEP). Ozone only assimilation improves winds (WEP = 46% for EnKF-uv, and 58% for EnKF-ψχ), but suffers from spurious gravity wave generation. Application of nonlinear normal mode initialization (NMI) greatly reduces the unwanted imbalance and increases the WEP for EnKF-uv (84%) and EnKF-ψχ (81%). Assimilation of only height observations also improved the winds (WEP = 60% for EnKF-uv, and 69% for EnKF-ψχ), with much less imbalance compared to the ozone experiment. The assimilation of both height and ozone performed the best, with WEP increasing to ~87% (~90% with NMI) for both EnKF-uv and EnKF-ψχ, demonstrating that wind extraction from ozone assimilation can be beneficial even in a data-rich environment. Ozone assimilation particularly improves the tropical winds, which are not well constrained by height observations due to lack of geostrophy.
Large eddy simulation of ship tracks in the collapsed marine boundary layer: a case study from the Monterey area ship track experiment

For the first time, a large eddy simulation (LES) coupled to a bulk aerosol scheme is used to simulate an aircraft-sampled ship track. The track was formed by the M/V Sanko Peace on 13 June 1994 in a shallow drizzling boundary layer with high winds but very low background aerosol concentrations (10 cm−3). A Lagrangian framework is used to simulate the evolution of a short segment of track as it is advected away from the ship for 8 h (a downwind distance exceeding 570 km). Using aircraft observations for initialization, good agreement is obtained between the simulated and observed features of the ambient boundary layer outside the track, including the organization of the cloud into mesoscale rolls. After 8 h, a line of aerosol is injected to start the ship track. The simulation successfully reproduces the significant albedo enhancement and suppression of drizzle observed within the track. The aerosol concentration within the track dilutes as it broadens due to turbulent mixing. A sensitivity study shows the broadening rate strongly depends on the alignment between the track and the wind-aligned boundary layer rolls, as satellite images of ship tracks suggest. Entrainment is enhanced within the simulated track, but the observed 100 m elevation of the ship track above the surrounding layer is not simulated, possibly because the LES quickly sharpens the rather weak observed inversion. Liquid water path within the simulated track increases with time even as the ambient liquid water path is decreasing. The albedo increase in the track from liquid water and cloud fraction enhancement (second indirect effect) eventually exceeds that from cloud droplet number increases (first indirect or Twomey effect). In a sensitivity study with a higher initial ambient aerosol concentration, stronger ship track aerosol source, and much weaker drizzle, there is less liquid water inside the track than outside for several hours downwind, consistent with satellite estimates for such situations. In that case, the Twomey effect dominates throughout, although, as seen in satellite images, the albedo enhancement of the track is much smaller.
Ocean mediation of tropospheric response to reflecting and absorbing aerosols

Radiative forcing by reflecting (e.g., sulfate, SO4) and absorbing (e.g., black carbon, BC) aerosols is distinct: the former cools the planet by reducing solar radiation at the top of the atmosphere and the surface, without largely affecting the atmospheric column, while the latter heats the atmosphere directly. Despite the fundamental difference in forcing, here we show that the structure of the tropospheric response is remarkably similar between the two types of aerosols, featuring a deep vertical structure of temperature change (of opposite sign) at the Northern Hemisphere (NH) mid-latitudes. The deep temperature structure is anchored by the slow response of the ocean, as a large meridional sea surface temperature (SST) gradient drives an anomalous inter-hemispheric Hadley circulation in the tropics and induces atmospheric eddy adjustments at the NH mid-latitudes. The tropospheric warming in response to projected future decline in reflecting aerosols poses additional threats to the stability of mountain glaciers in the NH. Additionally, robust tropospheric response is unique to aerosol forcing and absent in the CO2 response, which can be exploited for climate change attribution.
Drivers of the tropospheric ozone budget throughout the 21st century under the medium-high climate scenario RCP 6.0

Because tropospheric ozone is both a greenhouse gas and harmful air pollutant, it is important to understand how anthropogenic activities may influence its abundance and distribution through the 21st century. Here, we present model simulations performed with the chemistry–climate model SOCOL, in which spatially disaggregated chemistry and transport tracers have been implemented in order to better understand the distribution and projected changes in tropospheric ozone. We examine the influences of ozone precursor emissions (nitrogen oxides (NOx), carbon monoxide (CO) and volatile organic compounds (VOCs)), climate change (including methane effects) and stratospheric ozone recovery on the tropospheric ozone budget, in a simulation following the climate scenario Representative Concentration Pathway (RCP) 6.0 (a medium-high, and reasonably realistic climate scenario). Changes in ozone precursor emissions have the largest effect, leading to a global-mean increase in tropospheric ozone which maximizes in the early 21st century at 23% compared to 1960. The increase is most pronounced at northern midlatitudes, due to regional emission patterns: between 1990 and 2060, northern midlatitude tropospheric ozone remains at constantly large abundances: 31% larger than in 1960. Over this 70-year period, attempts to reduce emissions in Europe and North America do not have an effect on zonally averaged northern midlatitude ozone because of increasing emissions from Asia, together with the long lifetime of ozone in the troposphere. A simulation with fixed anthropogenic ozone precursor emissions of NOx, CO and non-methane VOCs at 1960 conditions shows a 6% increase in global-mean tropospheric ozone by the end of the 21st century, with an 11 % increase at northern midlatitudes. This increase maximizes in the 2080s and is mostly caused by methane, which maximizes in the 2080s following RCP 6.0, and plays an important role in controlling ozone directly, and indirectly through its influence on other VOCs and CO. Enhanced flux of ozone from the stratosphere to the troposphere as well as climate change-induced enhancements in lightning NOx emissions also increase the tropospheric ozone burden, although their impacts are relatively small. Overall, the results show that under this climate scenario, ozone in the future is governed largely by changes in methane and NOx; methane induces an increase in tropospheric ozone that is approximately one-third of that caused by NOx. Climate impacts on ozone through changes in tropospheric temperature, humidity and lightning NOx remain secondary compared with emission strategies relating to anthropogenic emissions of NOx, such as fossil fuel burning. Therefore, emission policies globally have a critical role to play in determining tropospheric ozone evolution through the 21st century.